Self-reconstruction of catalysts during oxygen evolution reaction(OER)is crucial for the development of energy conversion technologies.However,the relationship between the specific atomic structure of pre-catalysts an...Self-reconstruction of catalysts during oxygen evolution reaction(OER)is crucial for the development of energy conversion technologies.However,the relationship between the specific atomic structure of pre-catalysts and their electrocatalytic behavior after reconstruction via dual-ion leaching has not been extensively researched.In this work,we design a highly effective non-noble metal OER catalyst with heterointerface through continuous self-reconstruction of Co_(2)(OH)_(3)Cl@NiMoO_(4)as pre-catalyst by a straightforward dual-ion(i.e.MoO_(4)^(2-)and Cl^(-))leaching.In-situ Raman and in-situ Fourier transform infrared(FT-IR)spectroscopy have precisely identified the progressive phase transformation of the pre-catalyst during self-reconstruction,which results in a stable heterojunction of CoOOH and NiOOH(CoOOH@NiOOH).Further calculations based on density functional theory(DFT)of CoOOH@NiOOH evident that more electrons will be aggregated in the Fermi level of Co.Notably,Gibbs free energy(ΔG)for different OER steps of CoOOH@NiOOH exhibit lower energy costs of all intermediates,implying the well catalytic properties.Ultimately,the catalyst derived from dual-ion leaching displays outstanding OER performance,characterized by an overpotential of 275 mV at a current density of 10 mA·cm^(-2)and exceptional stability over 12 h reaction.This work successfully paves a way of finding high-performance OER catalysts based on non-noble metal through dual-ion leaching during self-reconstruction.展开更多
基金supported by the National Key Research and Development Program of China(No.2023YFB3809301)the National Natural Science Foundation of China(Nos.61905183,52127816 and 51832004).
文摘Self-reconstruction of catalysts during oxygen evolution reaction(OER)is crucial for the development of energy conversion technologies.However,the relationship between the specific atomic structure of pre-catalysts and their electrocatalytic behavior after reconstruction via dual-ion leaching has not been extensively researched.In this work,we design a highly effective non-noble metal OER catalyst with heterointerface through continuous self-reconstruction of Co_(2)(OH)_(3)Cl@NiMoO_(4)as pre-catalyst by a straightforward dual-ion(i.e.MoO_(4)^(2-)and Cl^(-))leaching.In-situ Raman and in-situ Fourier transform infrared(FT-IR)spectroscopy have precisely identified the progressive phase transformation of the pre-catalyst during self-reconstruction,which results in a stable heterojunction of CoOOH and NiOOH(CoOOH@NiOOH).Further calculations based on density functional theory(DFT)of CoOOH@NiOOH evident that more electrons will be aggregated in the Fermi level of Co.Notably,Gibbs free energy(ΔG)for different OER steps of CoOOH@NiOOH exhibit lower energy costs of all intermediates,implying the well catalytic properties.Ultimately,the catalyst derived from dual-ion leaching displays outstanding OER performance,characterized by an overpotential of 275 mV at a current density of 10 mA·cm^(-2)and exceptional stability over 12 h reaction.This work successfully paves a way of finding high-performance OER catalysts based on non-noble metal through dual-ion leaching during self-reconstruction.